Charles Scott Sherrington (1857–1952) is widely acclaimed as the most important neurophysiologist in history. He became a legend in his own time, coined the term "synapse", and in 1932 received the Nobel Prize in medicine for his discoveries on the function of neurons. By the time he presented the Gifford Lectures 1937–38, he represented the best that science had to offer on behalf of the relationship of the mind to the natural world. The lectures, including one never publicly presented, were published as Man on His Nature (1941). Here neurology meets theology at the busy and often treacherous intersection of science and religion. Examining Sherrington's views in some detail, the standard rendering of Sherrington as a theist cannot be sustained by their contents; he ends up as at least a humanist and perhaps an atheist. Views by neurologists and philosophers of mind some seventy to eighty years later are compared and contrasted with Sherrington's. Although expectations of a materialist/reductionist answer to the mind/body problem have not been realized, neuroscientist Raymond Tallis appears as a parallel figure to Sherrington: both are clearly naturalistic humanists. A theistic response is presented addressing the mind/body problem from a hylomorphic process theology perspective, along with some comments regarding natural theology in general. In the end, this essay has two complementary aims: (1) to relocate Sherrington's neurotheology—if it can be called that—in a more appropriate historiographical category; and (2) to offer a viable answer to the mind/body problem. [ABSTRACT FROM AUTHOR]